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This work demonstrates the feasibility of binary liquid crystal (LC) alignments, in which two forms of LC alignment are in a single pixel or a specific area using a surface-treated alignment layer and a photoalignment film of the adsorption of azo dyes onto the polymer surface in azo dye-doped liquid crystals. Binary LC alignments that involve two of common LC alignments, which are homogeneous, homeotropic, hybrid, and twisted nematic alignments, are initially demonstrated. Then, a binary LC alignment that comprises hybrid and homeotropic alignments is adopted to fabricate a viewing-angle-dependent liquid crystal display, which displays two images by changing viewing angles.